Self-assembled vertically aligned metal-oxide (Ni-CeO2) nanocomposite thin films with novel multifunctionalities have been successfully deposited by a one-step growth method. The novel nanocomposite structures presents high-density Ni-nanopillars vertically aligned in a CeO2 matrix. Strong and anisotropic magnetic properties have been demonstrated, with a saturation magnetization (Ms) of ∼175 emu cm-3 and ∼135 emu cm-3 for out-of-plane and in-plane directions, respectively. Such unique vertically aligned ferromagnetic Ni nanopillars in the CeO2 matrix have been successfully incorporated in high temperature superconductor YBa2Cu3O7 (YBCO) coated conductors as effective magnetic flux pinning centers. The highly anisotropic nanostructures with high density vertical interfaces between the Ni nanopillars and CeO2 matrix also promote the mixed electrical and ionic conductivities out-of-plane and thus demonstrate great potential as nanocomposite anode materials for solid oxide fuel cells and other potential applications requiring anisotropic ionic transport properties.